A1 Journal article (refereed)
Polariton response in the presence of Brownian dissipation from molecular vibrations (2021)

Kansanen, K. S. U., Toppari, J. J., & Heikkilä, T. T. (2021). Polariton response in the presence of Brownian dissipation from molecular vibrations. Journal of Chemical Physics, 154(4), Article 044108. https://doi.org/10.1063/5.0036905

JYU authors or editors

Publication details

All authors or editors: Kansanen, Kalle S. U.; Toppari, J. Jussi; Heikkilä, Tero T.

Journal or series: Journal of Chemical Physics

ISSN: 0021-9606

eISSN: 1089-7690

Publication year: 2021

Publication date: 28/01/2021

Volume: 154

Issue number: 4

Article number: 044108

Publisher: American Institute of Physics

Publication country: United States

Publication language: English

DOI: https://doi.org/10.1063/5.0036905

Publication open access: Not open

Publication channel open access: 

Publication is parallel published (JYX): https://jyx.jyu.fi/handle/123456789/74020

Web address of parallel published publication (pre-print): https://arxiv.org/abs/2011.03421

Abstract

We study the elastic response of a stationarily driven system of a cavity field strongly coupled with molecular excitons, taking into account the main dissipation channels due to the finite cavity linewidth and molecular vibrations. We show that the frequently used coupled oscillator model fails in describing this response especially due to the non-Lorentzian dissipation of the molecules to their vibrations. Signatures of this failure are the temperature dependent minimum point of the polariton peak splitting, the uneven polariton peak height at the minimum splitting, and the asymmetric shape of the polariton peaks even at the experimentally accessed “zero-detuning” point. Using a rather generic yet representative model of molecular vibrations, we predict the polariton response in various conditions, depending on the temperature, molecular Stokes shift and vibration frequencies, and the size of the Rabi splitting. Our results can be used as a sanity check of the experiments trying to “prove” results originating from strong coupling, such as vacuum-enhanced chemical reaction rate.

Keywords: molecular physics; quantum physics; quasiparticles; polaritons

Free keywords: molecular vibrations

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Ministry reporting: Yes

Reporting Year: 2021

JUFO rating: 1